Modulating the MoS2 Edge Structures by Doping Transition Metals for Electrocatalytic CO2 Reduction

Two-dimensional transition metal dichalcogenides (TMDs) nanomaterials, such as MoS2 and WSe2, have proved to be promising electrocatalysts for CO2 reduction, in which the reduction product is CO with high selectivity. In order to improve the sluggish CO desorption process and the overall electrocatalytic performance, we have extensively explored the optimal dopants in MoS2 by high-throughput density functional theory (DFT) calculations and demonstrated the enhanced electrocatalytic activity. The dopants of V, Zr, and Hf into MoS2 could significantly promote the desorption of CO from the MoS2 edge, achieving the optimal performance for electrocatalytic CO2 reduction. Furthermore, the dopants locating close to the active Mo site is crucial to influence the catalytic activity, while the dopant concentration is not important. The modulating strategy we proposed here also applies to other TMDs materials for enhancing electrocatalytic activity.